D. Puerto

Dynamics of plasma formation, relaxation, and topography modification induced by femtosecond laser pulses in crystalline and amorphous dielectrics

We have studied plasma formation and relaxation dynamics along with the corresponding topography modifications in fused silica and sapphire induced by single femtosecond laser pulses (800 nm and 120 fs). These materials, representative of high bandgap amorphous and crystalline dielectrics, respectively, require nonlinear mechanisms to absorb the laser light. The study employed a femtosecond time-resolved microscopy technique that allows obtaining reflectivity and transmission images of the material surface at well-defined temporal delays after the arrival of the pump pulse which excites the dielectric material. The transient evolution of the free-electron plasma formed can be followed by combining the time-resolved optical data with a Drude model to estimate transient electron densities and skin depths. The temporal evolution of the optical properties is very similar in both materials within the first few hundred picoseconds, including the formation of a high reflectivity ring at about 7 ps. In contrast, at longer delays (100 ps–20 ns) the behavior of both materials differs significantly, revealing a longer lasting ablation process in sapphire. Moreover, transient images of sapphire show a concentric ring pattern surrounding the ablation crater, which is not observed in fused silica. We attribute this phenomenon to optical diffraction at a transient elevation of the ejected molten material at the crater border. On the other hand, the final topography of the ablation crater is radically different for each material. While in fused silica a relatively smooth crater with two distinct regimes is observed, sapphire shows much steeper crater walls, surrounded by a weak depression along with cracks in the material surface. These differences are explained in terms of the most relevant thermal and mechanical properties of the material. Despite these differences the maximum crater depth is comparable in both material at the highest fluences used (16 J/cm2). The evolution of the crater depth as a function of fluence can be described taking into account the individual bandgap of each material.

Plasma formation and structural modification below the visible ablation threshold in fused silica upon femtosecond laser irradiation

We have investigated the temporal and spatial evolution of the ablation process induced in fused silica upon irradiation with single 120fs laser pulses at 800nm. Time-resolved microscopy images of the surface reflectivity at 400nm reveal the existence of a transient plasma distribution with annular shape surrounding the visible ablation crater. The material in this annular zone shows an increased reflectivity after irradiation, consistent with a local refractive index increase of approximately 0.01. White light interferometry measurements indicate a shallow surface depression in this outer region, most likely due to material densification.

Ultrafast imaging of transient electronic plasmas produced in conditions of femtosecond waveguide writing in dielectrics

Femtosecond laser-induced plasmas in bulk dielectrics are imaged under waveguide writing conditions, for different polarizations, pulse durations, and processing depths, and their temporal evolution is measured using ultrafast pump-probe microscopy. The irradiation beam profile is elliptically shaped yielding a disklike focal volume. We demonstrate for doped phosphate glass that increasing the pulse duration improves the spatial distribution of deposited energy by minimizing beam filamentation and prefocal depletion effects. As a consequence, energy deposition in the desired volume is greatly enhanced. Our results identify key parameters for optimizing femtosecond laser processing of dielectrics and different strategies to minimize energy loss channels.

In situ assessment and minimization of nonlinear propagation effects for femtosecond-laser waveguide writing in dielectrics

The effect of nonlinear propagation on the shape of the focal volume has been assessed by in situ plasma emission imaging during the subsurface processing of a commercial phosphate glass. The sample was processed with an elliptically shaped femtosecond-laser beam at 1 kHz repetition rate and scanned transversely with respect to the writing beam axis. As a consequence, optimal conditions for minimizing undesirable nonlinear propagation effects during the production of optical waveguides by direct laser writing have been determined. Under these conditions, it is possible to induce structural transformations and still preserve the focal volume shape associated with the linear propagation regime. While at low pulse energy a single scan laser-written structure does not support a guided mode, the use of multiple scans with minimized nonlinear propagation effects enables the production of optical waveguides. The latter show a significantly improved performance in terms of the refractive index change and propagation losses when compared to single scan waveguides.

Ultraviolet optical near-fields of microspheres imprinted in phase change films

We report an experimental method for directly imaging optical near-fields of dielectric microspheres upon illumination with ultraviolet nanosecond laser pulses. The intensity distribution is imprinted in chalcogenide films leaving behind a characteristic fingerprint with features below 200 nm in size, which we read out with high-resolution field emission scanning electron microscopy. The experimental results are well matched by a rigorous solution of Maxwell’s equations. Compared to previous works using infrared femtosecond laser pulses, the use of ultraviolet nanosecond pulses is identified to be superior in terms of minimum recordable features size and surface roughness of the imprint.

Femtosecond laser-controlled self-assembly of amorphous-crystalline nanogratings in silicon

Self-assembly (SA) of molecular units to form regular, periodic extended structures is a powerful bottom-up technique for nanopatterning, inspired by nature. SA can be triggered in all classes of solid materials, for instance, by femtosecond laser pulses leading to the formation of laser-induced periodic surface structures (LIPSS) with a period slightly shorter than the laser wavelength. This approach, though, typically involves considerable material ablation, which leads to an unwanted increase of the surface roughness. We present a new strategy to fabricate high-precision nanograting structures in silicon, consisting of alternating amorphous and crystalline lines, with almost no material removal. The strategy can be applied to static irradiation experiments and can be extended into one and two dimensions by scanning the laser beam over the sample surface. We demonstrate that lines and areas with parallel nanofringe patterns can be written by an adequate choice of spot size, repetition rate and scan velocity, keeping a constant effective pulse number (N eff) per area for a given laser wavelength. A deviation from this pulse number leads either to inhomogeneous or ablative structures. Furthermore, we demonstrate that this approach can be used with different laser systems having widely different wavelengths (1030 nm, 800 nm, 400 nm), pulse durations (370 fs, 100 fs) and repetition rates (500 kHz, 100 Hz, single pulse) and that the grating period can also be tuned by changing the angle of laser beam incidence. The grating structures can be erased by irradiation with a single nanosecond laser pulse, triggering recrystallization of the amorphous stripes. Given the large differences in electrical conductivity between the two phases, our structures could find new applications in nanoelectronics.

Independent control of beam astigmatism and ellipticity using a SLM for fs-laser waveguide writing

We have used a low repetition rate (1 kHz), femtosecond laser amplifier in combination with a spatial light modulator (SLM) to write optical waveguides with controllable cross-section inside a phosphate glass sample. The SLM is used to induce a controllable amount of astigmatism in the beam wavefront while the beam ellipticity is controlled through the propagation distance from the SLM to the focusing optics of the writing set-up. The beam astigmatism leads to the formation of two separate disk-shaped foci lying in orthogonal planes. Additionally, the ellipticity has the effect of enabling control over the relative peak irradiances of the two foci, making it possible to bring the peak irradiance of one of them below the material transformation threshold. This allows producing a single waveguide with controllable cross-section. Numerical simulations of the irradiance distribution at the focal region under different beam shaping conditions are compared to in situ obtained experimental plasma emission images and structures produced inside the glass, leading to a very satisfactory agreement. Finally, guiding structures with controllable cross-section are successfully produced in the phosphate glass using this approach.

Fabrication of amorphous micro-ring arrays in crystalline silicon using ultrashort laser pulses

We demonstrate a simple way to fabricate amorphous micro-rings in crystalline silicon using direct laser writing. This method is based on the fact that the phase of a thin surface layer can be changed into the amorphous phase by irradiation with a few ultrashort laser pulses (800 nm wavelength and 100 fs duration). Surface-depressed amorphous rings with a central crystalline disk can be fabricated without the need for beam shaping, featuring attractive optical, topographical, and electrical properties. The underlying formation mechanism and phase change pathway have been investigated by means of fs-resolved microscopy, identifying fluence-dependent melting and solidification dynamics of the material as the responsible mechanism. We demonstrate that the lateral dimensions of the rings can be scaled and that the rings can be stitched together, forming extended arrays of structures not limited to annular shapes. This technique and the resulting structures may find applications in a variety of fields such as ...

Coherent scatter-controlled phase-change grating structures in silicon using femtosecond laser pulses

Periodic structures of alternating amorphous-crystalline fringes have been fabricated in silicon using repetitive femtosecond laser exposure (800 nm wavelength and 120 fs duration). The method is based on the interference of the incident laser light with far- and near-field scattered light, leading to local melting at the interference maxima, as demonstrated by femtosecond microscopy. Exploiting this strategy, lines of highly regular amorphous fringes can be written. The fringes have been characterized in detail using optical microscopy combined modelling, which enables a determination of the three-dimensional shape of individual fringes. 2D micro-Raman spectroscopy reveals that the space between amorphous fringes remains crystalline. We demonstrate that the fringe period can be tuned over a range of 410 nm – 13 µm by changing the angle of incidence and inverting the beam scan direction. Fine control over the lateral dimensions, thickness, surface depression and optical contrast of the fringes is obtained via adjustment of pulse number, fluence and spot size. Large-area, highly homogeneous gratings composed of amorphous fringes with micrometer width and millimeter length can readily be fabricated. The here presented fabrication technique is expected to have applications in the fields of optics, nanoelectronics, and mechatronics and should be applicable to other materials.

Femtosecond-resolved ablation dynamics of Si in the near field of a small dielectric particle

Summary In this work we analyze the ablation dynamics of crystalline Si in the intense near field generated by a small dielectric particle located at the material surface when being irradiated with an infrared femtosecond laser pulse (800 nm, 120 fs). The presence of the particle (7.9 μm diameter) leads to a strong local enhancement (ca. 40 times) of the incoming intensity of the pulse. The transient optical response of the material has been analyzed by means of fs-resolved optical microscopy in reflection configuration over a time span from 0.1 ps to about 1 ns. Characteristic phenomena like electron plasma formation, ultrafast melting and ablation, along with their characteristic time scales are observed in the region surrounding the particle. The use of a time resolved imaging technique allows us recording simultaneously the material response at ordinary and large peak power densities enabling a direct comparison between both scenarios. The time resolved images of near field exposed regions are consistent with a remarkable temporal shift of the ablation onset which occurs in the sub-picosend regime, from about 500 to 800 fs after excitation.